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Title: Lattice doping regulated interfacial reactions in cathode for enhanced cycling stability

Abstract

Interfacial reactions between electrode and electrolyte are critical, either beneficial or detrimental, for the performance of rechargeable batteries. The general approaches of controlling interfacial reactions are either applying a coating layer on cathode or modifying the electrolyte chemistry. Here we demonstrate an approach of modification of interfacial reactions through dilute lattice doping for enhanced battery properties. Using atomic level imaging, spectroscopic analysis and density functional theory calculation, we reveal aluminum dopants in lithium nickel cobalt aluminum oxide are partially dissolved in the bulk lattice with a tendency of enrichment near the primary particle surface and partially exist as aluminum oxide nano-islands that are epitaxially dressed on the primary particle surface. The aluminum concentrated surface lowers transition metal redox energy level and consequently promotes the formation of a stable cathode-electrolyte interphase. The present observations demonstrate a general principle as how the trace dopants modify the solid-liquid interfacial reactions for enhanced performance.

Authors:
 [1];  [2];  [3];  [3]; ORCiD logo [4]; ORCiD logo [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Science Lab
  2. Univ. of Texas, Austin, TX (United States). McKetta Dept. of Chemical Engineering & Texas Materials Inst.
  3. Univ. of Pittsburgh, Pittsburgh, PA (United States). Dept. of Mechanical Engineering and Materials Science
  4. Univ. of Texas, Austin, TX (United States). Materials Science and Engineering Program and Texas Materials Inst.
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1571502
Report Number(s):
PNNL-SA-144976
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING

Citation Formats

Zou, Lianfeng, Li, Jianyu, Liu, Zhenyu, Wang, Guofeng, Manthiram, Arumugam, and Wang, Chongmin. Lattice doping regulated interfacial reactions in cathode for enhanced cycling stability. United States: N. p., 2019. Web. doi:10.1038/s41467-019-11299-2.
Zou, Lianfeng, Li, Jianyu, Liu, Zhenyu, Wang, Guofeng, Manthiram, Arumugam, & Wang, Chongmin. Lattice doping regulated interfacial reactions in cathode for enhanced cycling stability. United States. doi:10.1038/s41467-019-11299-2.
Zou, Lianfeng, Li, Jianyu, Liu, Zhenyu, Wang, Guofeng, Manthiram, Arumugam, and Wang, Chongmin. Thu . "Lattice doping regulated interfacial reactions in cathode for enhanced cycling stability". United States. doi:10.1038/s41467-019-11299-2. https://www.osti.gov/servlets/purl/1571502.
@article{osti_1571502,
title = {Lattice doping regulated interfacial reactions in cathode for enhanced cycling stability},
author = {Zou, Lianfeng and Li, Jianyu and Liu, Zhenyu and Wang, Guofeng and Manthiram, Arumugam and Wang, Chongmin},
abstractNote = {Interfacial reactions between electrode and electrolyte are critical, either beneficial or detrimental, for the performance of rechargeable batteries. The general approaches of controlling interfacial reactions are either applying a coating layer on cathode or modifying the electrolyte chemistry. Here we demonstrate an approach of modification of interfacial reactions through dilute lattice doping for enhanced battery properties. Using atomic level imaging, spectroscopic analysis and density functional theory calculation, we reveal aluminum dopants in lithium nickel cobalt aluminum oxide are partially dissolved in the bulk lattice with a tendency of enrichment near the primary particle surface and partially exist as aluminum oxide nano-islands that are epitaxially dressed on the primary particle surface. The aluminum concentrated surface lowers transition metal redox energy level and consequently promotes the formation of a stable cathode-electrolyte interphase. The present observations demonstrate a general principle as how the trace dopants modify the solid-liquid interfacial reactions for enhanced performance.},
doi = {10.1038/s41467-019-11299-2},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {8}
}

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